Electro-hydrodynamic processing, comprising electrospinning and electrospraying techniques, is a novel technology used in the production of nano- and sub-micro-scale materials with specific properties suitable for environmental remediation processes. Polycaprolactone (PCL) micro-fibrous mats and alginate microcapsules were produced using electrospinning and electrospraying techniques respectively, and Lysinibacillus sphaericus CBAM5, a bacterium capable of metal removal by adsorption and accumulation inside the cell, was immobilized in these matrices. The polymeric structure was able to protect and maintain cell viability and the bio-composite materials were used to capture gold from synthetic water samples. The micro-fibrous membranes with immobilized bacteria were able to remove 93% of the gold after 120 h of inclusion in the aqueous medium. Using a filtration system, an efficiency of 64% was obtained for the removal of the precious metal after 10 cycles of filtration (2 h of exposure to the gold solution). In contrast, the microencapsulated L. sphaericus CBAM5 captured 64% of the gold after 4 h of the assay. Thus, both micro-structured matrices were suitable for the immobilization and protection of L. sphaericus CBAM5 and they showed high efficiencies of gold biosorption. Hence, these bio-composite materials could be used to concentrate gold from industrial wastewaters.